EP3190652B1 - Ensemble d'électrodes à sécurité améliorée, son procédé de fabrication et élément électrochimique comprenant l'ensemble d'électrodes - Google Patents

Ensemble d'électrodes à sécurité améliorée, son procédé de fabrication et élément électrochimique comprenant l'ensemble d'électrodes Download PDF

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EP3190652B1
EP3190652B1 EP15868161.9A EP15868161A EP3190652B1 EP 3190652 B1 EP3190652 B1 EP 3190652B1 EP 15868161 A EP15868161 A EP 15868161A EP 3190652 B1 EP3190652 B1 EP 3190652B1
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coating layer
porous coating
electrode
organic
inorganic
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EP3190652A4 (fr
EP3190652A1 (fr
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Joo-Sung Lee
Sun-Mi Jin
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LG Chem Ltd
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LG Chem Ltd
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    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
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    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
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    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
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    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
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    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to an electrode assembly with improved safety, a manufacturing method therefor and an electrochemical device including the electrode assembly, and more particularly, to an electrode assembly with improved heat resistance and safety at high temperature in which an inorganic porous coating layer is formed on the surface of an electrode active material layer of one of a positive electrode and a negative electrode and an organic porous coating layer is formed on the surface of the other electrode active material layer, and the porous coating layer acts as a separator, eliminating the need for a separator, and an a manufacturing method therefor and an electrochemical device including the electrode assembly.
  • lithium ion batteries developed in the early 1990's have drawn particular attention due to their advantages in terms of higher operating voltages and much higher energy densities than traditional batteries using an aqueous electrolyte solution, for example, Ni-MH, Ni-Cd, and lead-acid batteries.
  • aqueous electrolyte solution for example, Ni-MH, Ni-Cd, and lead-acid batteries.
  • lithium ion batteries have safety issues, such as fires and explosions, caused by the use of organic electrolytes, and their disadvantage is complex manufacturing.
  • lithium ion batteries and lithium ion polymer batteries generally have a polyolefin based separator to prevent a short circuit between a positive electrode and a negative electrode.
  • the downside of the polyolefin based separator is that the separator returns to its original size by thermal contraction at high temperature due to the properties of the separator material, for example, the properties of polyolefins that generally melt at 200°C or less and processing properties, for example, property to undergo a stretching process for adjusting the pore size and porosity. Accordingly, when battery temperature increases due to internal/external impacts, the separator contracts or melts and there is a high likelihood that a short circuit will occur between positive and negative electrodes, hence the batteries have a high risk of explosions caused by emission of electrical energy.
  • WO 2014/071144 A1 discloses an integrated electrode separator consisting of an electrode coated with a porous coating, whereby the porous coating is an organic porous coating or an inorganic porous coating.
  • US 2012/034509 A1 discloses an electrochemical device that comprises an electrode assembly that includes a cathode, an anode and a porous separator that includes a monolayer-type polyolefin-based microporous film and a porous coating layer made of inorganic particles with average diameter of 0.001-10 ⁇ m and having a dielectric constant of 5 or more.
  • US 2012/196191 A1 discloses an electrochemical device that comprises an electrode assembly that includes a cathode, an anode and a separator, whereby the separator is composed of two layers: an organic porous substrate and a porous coating layer made of inorganic particles with a dielectric constant of 5 or more.
  • DE 11 2011 105 969 T5 discloses an electrochemical device that comprises an electrode assembly that has stacked in sequential order: a positive current collector; a positive active material layer; a porous inorganic coating; a porous organic coating; a negative active material layer, and a negative current collector, whereby the inorganic porous coating is coated on the negative electrode before the assembly of the electrodes.
  • US 2012/231321 A1 discloses an electrochemical device that comprises an electrode assembly that includes a cathode, and anode an a porous bilayer separator, whereby the separator is composed of two layers: a porous substrate and a porous coating layer made of inorganic ceramic particles and is sandwiched between the two electrodes.
  • US 2010/316903 A1 discloses an electrochemical device that comprises an electrode assembly that includes a cathode, an anode and a porous separator that includes a monolayer-type polyolefin-based porous film and a porous coating layer made of inorganic particles having a dielectric constant of 5 or more.
  • the present disclosure is directed to providing an electrode assembly that is tightly adhered at the electrode interface, is less likely to have thermal contraction, and provides a shut down function, and a manufacturing method therefor and an electrochemical device including the electrode assembly.
  • an electrode assembly comprising: a positive electrode composed of a positive electrode current collector, a positive electrode active material layer, and a porous coating layer stacked in a sequential order; and a negative electrode composed of a negative electrode current collector, a negative electrode active material layer, and a porous coating layer stacked in a sequential order, wherein one of the porous coating layer at the positive electrode and the porous coating layer at the negative electrode is an organic porous coating layer, and the other is an inorganic porous coating layer, and wherein the organic porous coating layer is free of inorganic particles and includes spherical particles formed from at least one selected from the group consisting of high density polyethylene, low density polyethylene, linear low density polyethylene, polypropylene, high crystalline polypropylene, polyethylene-propylene copolymer, polyethylene-butylene copolymer, polyethylene-hexene copolymer, polyethylene-octene copolymer, polystyrene-butylene-st
  • the organic porous coating layer may be formed in an amount of between 0.1 and 7 g/m 2 over the entire surface of the active material layer of the positive electrode or the negative electrode.
  • the organic porous coating layer is formed with a uniform thickness in an amount of between 0.1 and 7 g/m 2 over the entire surface of the active material layer of the positive electrode or the negative electrode, to shut down the battery in the event of abnormal heat generation.
  • the inorganic porous coating layer may include inorganic particles having a dielectric constant of 5 or higher, inorganic particles having an ability to transport lithium ions, or their mixtures.
  • the inorganic particles having a dielectric constant of 5 or higher may be BaTiO 3 , Pb(Zr,Ti)O 3 (PZT), Pb 1-x La x Zr 1-y Ti y O 3 (PLZT), PB(Mg 1/3 Nb 2/3 )O 3 -PbTiO 3 (PMN-PT), hafnia (HfO 2 ), SrTiO 3 , SnO 2 , CeO 2 , MgO, NiO, CaO, ZnO, ZrO 2 , Y 2 O 3 , Al 2 O 3 , TiO 2 , or their mixtures.
  • the inorganic particles having an ability to transport lithium ions may be lithium phosphate (Li 3 PO 4 ), lithium titanium phosphate (Li x Ti y (PO 4 ) 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 3), lithium aluminum titanium phosphate (Li x Al y Ti z (PO 4 ) 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 1, 0 ⁇ z ⁇ 3), (LiAlTiP) x Oy based glass (0 ⁇ x ⁇ 4, 0 ⁇ y ⁇ 13), lithium lanthanum titanate (Li x La y TiO 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 3), lithium germanium thiophosphate (Li x Ge y P z S w , 0 ⁇ x ⁇ 4, 0 ⁇ y ⁇ 1, 0 ⁇ z ⁇ 1, 0 ⁇ w ⁇ 5),
  • the inorganic porous coating layer may be formed in an amount of between 1 and 30 g/m 2 on a surface of the electrode.
  • the inorganic particles may have a diameter in a range of between 0.1 and 1.0 ⁇ m, and the organic particles may have a diameter in a range of between 0.05 and 1.0 ⁇ m.
  • an electrochemical device including the aforesaid electrode assembly, and the electrochemical device may be a lithium secondary battery.
  • a method for manufacturing an electrode assembly comprising: (a) applying a mixed electrode slurry to a current collector to manufacture an electrode; (b) preparing a slurry including inorganic particles, and coating the slurry on a surface of an electrode active material layer of the electrode and drying to form an inorganic porous coating layer; (c) applying a mixed electrode slurry to a current collector to manufacture another electrode; (d) preparing a slurry including organic particles, free of inorganic particles, and that includes spherical particles, and coating the slurry on a surface of an electrode active material layer of the other electrode and drying to form an organic porous coating layer; and e) stacking the electrodes such that the inorganic porous coating layer and the organic porous coating layer face each other.
  • a lamination process may be performed at a temperature in the range of between 30 and 150°C and a pressure in the range of between 98,000 and 490,000 N/cm 2 for bonding between the porous coating layer and the electrode.
  • the electrode assembly according to the present disclosure eliminates the need for a general separator because the electrode acts as a separator.
  • the mechanical properties and ionic conductivity of the inorganic porous coating layer and the organic porous coating layer are superior, contributing to the performance improvement of electrochemical devices.
  • an electrode assembly in which an inorganic porous coating layer or an organic porous coating layer are formed on the surface of each of a positive electrode and a negative electrode and the inorganic porous coating layer and the organic porous coating layer are assembled facing each other, and an electrochemical device including the electrode assembly.
  • an electrode assembly A is considered, and it is configured such that a negative electrode active material layer 2 is formed on a negative electrode current collector 1, an organic porous coating layer 3 is formed on the surface of the negative electrode active material layer 2, a positive electrode active material layer 2' is formed on a positive electrode current collector 1', an inorganic porous coating layer 3' is formed on the surface of the positive electrode active material layer 2', and the organic porous coating layer 3 and the inorganic porous coating layer 3' face each other.
  • the present disclosure provides a method for manufacturing an electrode assembly according to claim 9.
  • the electrode assembly according to the present disclosure is characterized by providing an integrated electrode of new concept integrating the function of a general separator serving as a spacer which allows ions to pass through while preventing the electronic contact between the positive electrode and the negative electrode and the function of an electrode where reversible lithium intercalation and deintercalation takes place.
  • the electrode assembly of an integrated separator/electrode type has an inorganic porous coating layer or an organic porous coating layer formed on the surface of the positive electrode having the positive electrode active material layer.
  • an inorganic porous coating layer is formed on the surface of the positive electrode active material layer
  • an organic porous coating layer is formed on the surface of the negative electrode active material layer
  • an inorganic porous coating layer is formed on the surface of the negative electrode active material layer.
  • the inorganic porous coating layer and the organic porous coating layer face each other.
  • the organic porous coating layer and the inorganic porous coating layer formed on the surface of the active material layers of each of the positive electrode and the negative electrode may be stacked facing each other without forming a separate binder layer.
  • the organic porous coating layer is free of inorganic particles. If inorganic particles are included in the organic porous coating layer, the battery does not fully shut down when overheated, failing to ensure safety and causing a reduction in bonding with the inorganic porous coating layer.
  • the inorganic porous coating layer may have a uniform pore structure in which inorganic particles are packed closely and held together by organic binder polymer to form 'interstitial volume' structure between the inorganic particles.
  • the organic porous coating layer has a uniform pore structure because interstitial volume structure is formed between organic particles.
  • the organic porous coating is free of inorganic particles, and one of the components that make up the organic porous coating layer is organic particles.
  • the organic particles shut down by pore blocking when the temperature of the battery is abnormally high.
  • the organic particles preferably has a melting point of between 100 and 180°C. If the organic particles have a melting point of less than 100°C. the shutdown temperature of the organic porous coating layer is too low, and when an electrochemical device is repeatedly used, an unintentional shut down takes place, causing an increase of impedance. On the contrary, if the melting point of the organic particles is higher than 180°C, the shut down function is not fully obtained, and thermal runaway occurs when the temperature increases.
  • the organic particles have a particle shape having the mean particle size D50 of 0.01 ⁇ 5.0 ⁇ m, more preferably the mean particle size D50 of 0.03 ⁇ 3.0 ⁇ m, and particularly preferably the mean particle size D50 of 0.05 ⁇ 1.0 ⁇ m, in terms of allowing an electrolyte solution to penetrate into the organic particles as an active material layer and preventing the impedance increase.
  • the particle shape is spherical in terms of allowing for a uniform pore structure due to 'interstitial volume' structure formed between organic particles packed closely and held together by organic binder polymer.
  • 'spherical' does not refer to only a perfect spherical shape, and encompasses a particle shape which is close to a spherical shape or capable of forming 'interstitial volumes' or pores. Furthermore, to maintain the particle shape even after applied on the electrode, the organic particles should not be swollen or dispersed in an organic solvent.
  • the organic porous coating layer may be formed over the entire electrode surface in an amount of between 0.1 and 7 g/m 2 , and when the amount used lies within the numerical range, it is possible to ensure safety of the battery at high temperature while not causing significant degradation of the battery performance.
  • the organic porous coating layer and the inorganic porous coating layer are coated on the active material layers of each of the positive electrode and the negative electrode such that the organic porous coating layer and the inorganic porous coating layer face each other.
  • the inorganic particles are not particularly limited so long as they can prevent a short circuit between the negative electrode and the positive electrode and are electrochemically stable. That is, the inorganic particles that can be used in the present disclosure are not particularly limited if they do not cause any oxidation and/or reduction reaction in the operating voltage range (for example, 0 ⁇ 5V for Li/Li + ) of the battery used. Particularly, the use of inorganic particles having the ability to transport ions increases ionic conductivity in electrochemical devices, contributing to the performance improvement, and accordingly, those having ionic conductivity that is as high as possible are desirable.
  • the inorganic particles having high density are difficult to disperse in the coating process and have a problem of increased weight in the manufacture of the battery, and accordingly, those having density that is as low as possible are desirable.
  • the use of an inorganic material having a high dielectric constant contributes to the increase in dissolution rate of electrolyte salts, for example, lithium salts, in a liquid electrolyte, thereby increasing ionic conductivity of an electrolyte solution.
  • the inorganic particles are preferably inorganic particles having a dielectric constant of 5 or higher, inorganic particles having the ability to transport lithium ions, or their mixtures.
  • Non-limiting examples of the inorganic particles having a dielectric constant of 5 or higher include BaTiO3, Pb(Zr,Ti)O 3 (PZT), Pb 1-x La x Zr 1-y Ti y O 3 (PLZT), PB(Mg 1/3 Nb 2/3 )O 3 -PbTiO 3 (PMN-PT), hafnia (HfO 2 ), SrTiO 3 , SnO 2 , CeO 2 , MgO, NiO, CaO, ZnO, ZrO 2 , Y 2 O 3 , Al 2 O 3 , TiO 2 , or their mixtures.
  • the inorganic particles having the ability to transport lithium ions as used herein refer to inorganic particles which contain lithium atoms but do not store lithium, and have a function to move lithium ions, and because the inorganic particles having the ability to transport lithium ions can transfer and move lithium ions due to a kind of defect present in the particle structure, it is possible to improve lithium ionic conductivity in the battery, contributing to the improvement of the battery performance.
  • Non-limiting examples of the inorganic particles having the ability to transport lithium ions include lithium phosphate (Li 3 PO 4 ), lithium titanium phosphate (Li x Ti y (PO 4 ) 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 3), lithium aluminum titanium phosphate (Li x Al y Ti z (PO 4 ) 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 1, 0 ⁇ z ⁇ 3), (LiAlTiP) x O y based glass (0 ⁇ x ⁇ 4, 0 ⁇ y ⁇ 13) such as 14Li 2 O-9Al 2 O 3 -38TiO 2 -39P 2 O 5 , lithium lanthanum titanate (Li x La y TiO 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 3), lithium germanium thiophosphate (Li x Ge y P z S w , 0
  • the inorganic particles having high dielectric properties i.e., Pb(Zr,Ti)O 3 (PZT), Pb 1-x La x Zr 1-y Ti y O 3 (PLZT), PB(Mg 1/3 Nb 2/3 )O 3 -PbTiO 3 (PMN-PT), and hafnia (HfO 2 ) exhibit high dielectric properties of a dielectric constant of 100 or higher, as well as piezoelectricity that is the appearance of a potential difference across two surfaces due to electric charge generated when stretched or compressed by the application of predetermined pressure, thereby preventing the occurrence of an internal short circuit between two electrodes caused by external impacts, ultimately contributing to the improvement of safety of the battery. Furthermore, when the high dielectric constant inorganic particles and the inorganic particles having the ability to transport lithium ions are used in combination, their synergistic effect can be greatly magnified.
  • the size of the inorganic particles preferably ranges from 0.001 to 10 ⁇ m or from 0.1 to 1.0 ⁇ m if possible.
  • the size of the inorganic particles is less than the lower limit, dispersion reduces, making it difficult to adjust the properties of the porous coating layer, and when the size of the inorganic particles exceeds the upper limit, a porous coating layer formed with the same solids content is thicker and has poorer mechanical properties, and there is a high probability that an internal short circuit will occur during charging or discharging of the battery due to too large pore size due to too large pore size.
  • the inorganic porous coating layer may be formed on the electrode surface in an amount of between 1 and 30 g/m 2 , and it is possible to ensure safety of the battery at high temperature while not causing significant degradation of the battery performance within the range.
  • One of the components that make up the organic porous coating layer and/or the inorganic porous coating layer may include organic binder polymer commonly used in the art.
  • the organic binder polymer When put in a solvent, the organic binder polymer is swollen or dispersed to form bonds between the inorganic particles, between the organic particles, between the inorganic particles and the electrode current collector, or between the organic particles and the electrode current collector.
  • the organic binder polymer may include organic binder polymers whose glass transition temperature T g is as low as possible, and preferably those having the glass transition temperature in the range of between -200 and 200°C. This is because it can improve the mechanical properties of a final coating layer such as flexibility and elasticity.
  • the organic binder polymer acts as a binder to connect and immobilize between the inorganic particles, between the organic particles, between the surfaces of the inorganic particles/organic particles and the electrode active material particles, and some pores in the electrode, thereby preventing the degradation of the mechanical properties of the electrode finally manufactured.
  • the organic binder polymer does not need to have the ability to transport ions, but the use of the organic binder polymer having the ability to transport ions can further improve the performance of electrochemical devices. Accordingly, the organic binder polymer preferably has a dielectric constant that is as high as possible.
  • the organic binder polymer may have a property to exhibit high degree of swelling in an electrolyte solution by gelation when swollen in a liquid electrolyte solution.
  • Non-limiting examples of the organic binder polymer that can be used in the present disclosure include polyethylene oxide, polyvinylidene fluoride, polyvinylidene fluoride-hexafluoropropylene, polyvinylidene fluoride-trichloroethylene, polymethylmethacrylate, polyacrylonitrile, polyacrylonitrile-styrene copolymer, polyvinylchloride (PVC), polyvinylpyrrolidone, polyvinylacetate, polyethylene vinyl acetate copolymer, gelatin, cyanoethylpullulan, cyanoethylpolyvinylalcohol, cyanoethylcellulose, cyanoethylsucrose, pullulan, cellulose acetate, cellulose acetate butyrate, cellulose acetate propionate, polyethyleneglycol, glyme, polyethyleneglycol dimethylether, carboxymethyl cellulose, or their mixtures.
  • PVC polyvin
  • composition of the inorganic particles/organic particles and the organic binder polymer in the inorganic porous coating layer or the organic porous coating layer formed on the electrode according to the present disclosure can be adjusted based on the thickness and structure of a final coating layer. More specifically, it is preferred to adjust the ingredient ratio of the inorganic particles/organic particles and the organic binder polymer within the weight ratio range of between 10:90 and 99:1, preferably the weight ratio range of between 50:50 and 98:2.
  • a porous coating layer may be formed in which bonds are formed between the inorganic particles or the organic particles without using organic binder polymer according to the manufacturing method and/or the use of the battery.
  • the thickness of a porous coating layer formed by coating an inorganic particle slurry/organic particle slurry on the electrode surface is no limitation on the thickness of a porous coating layer formed by coating an inorganic particle slurry/organic particle slurry on the electrode surface, but the thickness of the porous coating layer can be adjusted in consideration of the battery performance, and thickness adjustment is independently accomplished in each of the positive electrode and the negative electrode.
  • the present disclosure preferably adjusts the thickness of the coating layer within the range of between 1 and 100 ⁇ m, and more preferably the range of between 1 and 30 ⁇ m.
  • the pore size and porosity of the porous coating layer is an important factor affecting ionic conductivity adjustment.
  • the pore size and porosity of the porous coating layer preferably ranges from 0.001 to 10 ⁇ m, and from 10 to 95%, respectively.
  • the porous coating layer formed on the electrode according to the present disclosure may further include additive.
  • manufacturing method includes (a) applying a mixed electrode slurry to a current collector to manufacture an electrode, (b) preparing a slurry for forming a porous coating layer including inorganic particles, and coating the slurry on the surface of one electrode active material layer and drying to form an inorganic porous coating layer, (c) applying a mixed electrode slurry to a current collector to manufacture another electrode, (d) preparing a slurry for forming a porous coating layer including organic particles, free of inorganic particles, and that includes spherical particles, and coating the slurry on the surface of the other electrode active material layer and drying to form an organic porous coating layer, and (e) stacking the electrodes such that the inorganic porous coating layer and the organic porous coating layer formed on the electrodes face each other.
  • a lamination process may be performed before the step (e) if necessary, to form bonds between the porous coating layer and the electrode.
  • the lamination is performed at temperature in the range of between 30 and 150°C and/or pressure in the range of between 98,000 and 490,000 N/cm 2 .
  • the solvent used in the porous coating layer slurry preferably has a solubility index similar to that of organic binder polymer to use, and a low boiling point. This is because it achieves uniform mixing, and facilitates the subsequent removal of the solvent.
  • Non-limiting examples of the solvent include acetone, tetrahydrofuran, methylene chloride, chloroform, dimethylformamide, N-methyl-2-pyrrolidone (NMP), cyclohexane, water, or their mixtures.
  • an optimal pulverization time is from 1 to 20 hours, and the pulverized inorganic particles/organic particles preferably have the aforesaid particle size.
  • the pulverization method includes common methods, and particularly preferably a ball mill method.
  • a method for coating the inorganic porous coating layer slurry or the organic porous coating layer slurry on the surface of each electrode active material layer includes common methods known in the art, for example, dip coating, die coating, roll coating, comma coating, or their combinations.
  • the porous coating layer slurry may be applied after the solvent in the electrode active material layer is fully dried, or the porous coating layer slurry may be applied when the active material layer is sticky due to the solvent remaining in the electrode active material layer, to ensure stronger bonds between the active material layer and the porous coating layer.
  • an electrochemical device including a positive electrode, a negative electrode, and an electrolyte solution
  • an electrochemical device including an electrode assembly composed of electrodes having a porous coating layer of inorganic particles/organic particles as an alternative to a separator on the surface of each of the positive electrode and the negative electrode.
  • the electrochemical device includes any type of device that undergoes electrochemical reactions, for example, any type of primary battery, secondary battery, fuel cell, solar cell, or capacitor.
  • an electrochemical device In a method for manufacturing an electrochemical device according to the invention using the electrodes manufactured as described above, a general separator is not used and only electrodes having a porous coating layer manufactured as described above are used, and an electrochemical device may be manufactured by assembling the electrodes through a winding or stacking process and injecting an electrolyte solution.
  • the electrode having the porous coating layer according to the present disclosure is not limited to a particular type, and may include electrodes manufactured such that an electrode active material is bonded to an electrode current collector by common methods known in the art.
  • the electrode active material non-limiting examples of the positive electrode active material include common positive electrode active materials used in the positive electrode of conventional electrochemical devices, and particularly preferably lithium intercalation materials such as lithium manganese oxide, lithium cobalt oxide, lithium nickel oxide, lithium iron oxide, or composite oxide thereof.
  • Non-limiting examples of the negative electrode active material include common negative electrode active materials used in the negative electrode of conventional electrochemical devices, and particularly preferably lithium intercalation materials such as lithium metal or lithium alloy, carbon, petroleum coke, activated carbon, graphite, or other carbons.
  • lithium intercalation materials such as lithium metal or lithium alloy, carbon, petroleum coke, activated carbon, graphite, or other carbons.
  • Non-limiting examples of the positive electrode current collector include foils manufactured by aluminum, nickel or their combinations
  • non-limiting examples of the negative electrode current collector include foils manufactured by copper, gold, nickel or copper alloy, or their combinations.
  • the electrolyte solution that can be used in the present disclosure includes, but is not limited to, electrolyte solutions in which a salt is dissolved or dissociated in an organic solvent, the salt having a structure represented by, for example, A + B - , wherein A + is an alkali metal cation such as Li + , Na + , K + , or their combinations, and B - is an anion such as PF 6 - , BF 4 - , Cl - , Br - , I - , ClO4 - , ASF 6 - , CH 3 CO 2 - , CF 3 SO 3 - , N(CF 3 SO 2 ) 2 - , C(CF 2 SO 2 ) 3 - , or their combinations, and the organic solvent includes propylene carbonate (PC), ethylene carbonate (EC), diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC), dimethyl sulfoxide, aceton
  • the injection of the electrolyte solution may be performed in any suitable step of a manufacturing process of an electrochemical device based on a manufacturing process and required properties of a final product. That is, the injection of the electrolyte solution may be performed before assembly of the electrochemical device or in the final step of assembly of the electrochemical device.
  • the electrode itself acts as a separator, eliminating the need for a separate separator used in conventional batteries.
  • An electrochemical device manufactured by the method is preferably a lithium secondary battery, and the lithium secondary battery includes lithium metal secondary batteries, lithium ion secondary batteries, lithium polymer secondary batteries, or lithium ion polymer secondary batteries.
  • 96 weight% of carbon powder as a negative electrode active material 3 weight% of polyvinylidene fluoride (PVdF) as a binder, and 1 weight% of carbon black as a conducting material were added to a solvent, N-methyl-2-pyrrolidone (NMP), to prepare a mixed negative electrode slurry.
  • the mixed negative electrode slurry was applied to a negative electrode current collector of copper (Cu) thin film with 10 ⁇ m thickness, and dried to manufacture a negative electrode having a negative electrode active material layer, followed by roll pressing.
  • PVdF-CTFE polyvinylidene fluoride-chlorotrifluoroethylene copolymer
  • the particle size of alumina in the prepared slurry can be controlled based on the size (particle size distribution) of beads used in the ball mill and the ball mill time, and in example 1, alumina was pulverized with the particle size of about 500 nm to prepare a slurry forming an inorganic porous coating layer. Subsequently, the slurry for forming an inorganic porous coating layer was coated on the surface of the positive electrode active material layer by a dip coating method, such that about 2g/m 2 of inorganic particles were formed on the positive electrode active material layer.
  • the organic porous coating layer of the negative electrode and the inorganic porous coating layer of the positive electrode manufactured as described above were assembled using a stacking method such that they face each other, and a general polyolefin based separator was not used.
  • EC ethylene carbonate
  • PC propylene carbonate
  • DEC diethyl carbonate
  • a lithium secondary battery was manufactured by the same method as example 1.
  • an electrode and a battery were manufactured by the same method as example 1.
  • lithium secondary battery having the battery capacity of 11.0 mAh prepared in examples 1 and 2 and comparative example 1 capacity was measured during charging and discharging at the discharge rate of 0.2C at room temperature, and its results were plotted as solid line graphs in FIGS. 2a to 2c . From this, it could be seen that the lithium secondary batteries of examples 1 and 2 and comparative example 1 all achieved the design level of capacity.
  • the lithium secondary batteries were kept at 130°C for 30 minutes, and after then, were discharged discharge rate of 0.2C again.
  • the lithium secondary batteries of examples 1 and 2 showed improved safety even when exposed to high temperature environment because charging and discharging was limited by a desired shut down effect, but it could be seen that the lithium secondary battery of comparative example 1 showed similar charging/discharging behaviors to those of room temperature (solid line graph) at high temperature (dashed line graph) of FIG. 2a , and safety of the lithium secondary battery was not improved.

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Claims (10)

  1. Ensemble électrode comprenant :
    une électrode positive composée d'un collecteur de courant d'électrode positive, d'une couche de matériau actif d'électrode positive et d'une couche de revêtement poreux, empilés dans un ordre séquentiel ; et
    une électrode négative composée d'un collecteur de courant d'électrode négative, d'une couche de matériau actif d'électrode négative et d'une couche de revêtement poreux, empilés dans un ordre séquentiel,
    caractérisé en ce que soit la couche de revêtement poreux à l'électrode positive, soit la couche de revêtement poreux à l'électrode négative est une couche de revêtement poreux organique, et l'autre est une couche de revêtement poreux inorganique, et
    dans lequel la couche de revêtement poreux organique est exempte de particules inorganiques et inclut des particules sphériques formées à partir d'au moins un élément sélectionné dans le groupe constitué de polyéthylène haute densité, polyéthylène faible densité, polyéthylène faible densité linéaire, polypropylène, polypropylène hautement cristallin, copolymère de polyéthylène-propylène, copolymère de polyéthylène-butylène, copolymère de polyéthylène-hexène, copolymère de polyéthylène-octène, copolymère de polystyrène-butylène-styrène, copolymère de polystyrène-éthylène-butylène-styrène, polystyrène, oxyde de polyphénylène, polysulfone, polycarbonate, polyester, polyamide, polyuréthane, polyacrylate, chlorure de polyvinylidène, polysiloxane, ionomère de polyoléfine, pentène polyméthylique, oligocyclopentadiène hydrogéné (HOCP), et leurs dérivés,
    la couche de revêtement poreux organique et la couche de revêtement poreux inorganique sont face l'une à l'autre.
  2. Ensemble électrode selon la revendication 1, dans lequel la couche de revêtement poreux organique est revêtue dans une quantité comprise entre 0,1 et 7 g/m2 sur une surface de la couche de matériau actif d'électrode.
  3. Ensemble électrode selon la revendication 1, dans lequel la couche de revêtement poreux inorganique inclut des particules inorganiques ayant une constante diélectrique égale ou supérieure à 5, les particules inorganiques ayant une capacité de transporter des ions de lithium, ou leurs mélanges.
  4. Ensemble électrode selon la revendication 3, dans lequel les particules inorganiques ayant une constante diélectrique égale ou supérieure à 5 sont BaTiO3, Pb(Zr,Ti)O3 (PZT), Pb1-xLaxZr1-yTiyO3 (PLZT), PB(Mg1/3Nb2/3O3 - PbTiO3(PMN-PT), hafnia (HfO2), SrTiO3, SnO2, CeO2, MgO, NiO, CaO, ZnO, ZrO2, Y2O3, Al2O3, TiO2, ou leurs mélanges.
  5. Ensemble électrode selon la revendication 3, dans lequel les particules inorganiques ayant une capacité à transporter des ions de lithium sont
    phosphate de lithium (Li3PO4),
    phosphate de lithium titane (LixTiv(PO4)3, 0 < x < 2, 0 < y < 3),
    phosphate de lithium aluminium titane (LixAlvTiz(PO4)3, 0 < x < 2, 0 < y < 1, 0 < z < 3),
    verre à base de (LiAlTiP)xOv (0 < x < 4, 0 < y < 13),
    titanate de lithium lanthane (LixLavTiO3, 0 < x < 2, 0 < y < 3),
    thiophosphate de lithium germanium (LixGevPzSw, 0 < x < 4, 0 < y < 1, 0 < z < 1, 0 < w < 5),
    nitrure de lithium (LixNy, 0 < x < 4, 0 < y < 2),
    verre à base de SiS2 (LixSiySz, 0 < x < 3, 0 < y < 3, 0 < z < 4),
    verre à base de P2S5 (LixPvSz, 0 < x < 3, 0 < y < 3, 0 < z < 7),
    ou leurs mélanges.
  6. Ensemble électrode selon la revendication 1, dans lequel la couche de revêtement poreux inorganique est revêtue dans une quantité comprise entre 1 et 30 g/m2, sur une surface de la couche de matériau actif d'électrode.
  7. Dispositif électrochimique comprenant l'ensemble électrode défini dans l'une quelconque des revendications 1 à 6,
  8. Dispositif électrochimique selon la revendication 7, dans lequel le dispositif électrochimique est une batterie rechargeable au lithium.
  9. Procédé de fabrication d'un ensemble électrode selon la revendication 1, consistant à :
    (a) appliquer une suspension d'électrode mélangée à un collecteur de courant pour fabriquer une électrode ;
    (b) préparer une suspension incluant des particules inorganiques, et enduire la suspension sur une surface d'une couche de matériau actif d'électrode de l'électrode et sécher pour former une couche de revêtement poreux inorganique ;
    (c) appliquer une suspension d'électrode mélangée à un collecteur de courant pour fabriquer une autre électrode ;
    (d) préparer une suspension incluant des particules organiques, exempte de particules inorganiques, et qui inclut des particules sphériques, et enduire la suspension sur une surface d'une couche de matériau actif d'électrode de l'autre électrode et sécher pour former une couche de revêtement poreux organique ; et
    e) empiler les électrodes de telle sorte que la couche de revêtement poreux inorganique et la couche de revêtement poreux organique sont face l'une à l'autre.
  10. Procédé de fabrication d'un ensemble électrode selon la revendication 9, dans lequel après l'étape (b) ou (d) et avant l'étape (e), un processus de stratification est effectué à une température comprise entre 30 et 150°C et à une pression comprise entre 98 000 et 490 000 N/cm2 pour une liaison entre la couche de revêtement poreux et l'électrode.
EP15868161.9A 2014-12-08 2015-12-08 Ensemble d'électrodes à sécurité améliorée, son procédé de fabrication et élément électrochimique comprenant l'ensemble d'électrodes Active EP3190652B1 (fr)

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US10629913B2 (en) 2020-04-21
EP3190652A4 (fr) 2017-09-13
KR20160069493A (ko) 2016-06-16
KR101734328B1 (ko) 2017-05-11
EP3190652A1 (fr) 2017-07-12
JP2018503933A (ja) 2018-02-08
CN107004808B (zh) 2019-11-12
US20170309915A1 (en) 2017-10-26
WO2016093589A1 (fr) 2016-06-16
JP6461328B2 (ja) 2019-01-30
CN107004808A (zh) 2017-08-01
PL3190652T3 (pl) 2020-02-28

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